Constrained TRPV1 agonists synthesized via silver-mediated intramolecular azo-methine ylide cycloaddition of α-iminoamides

Bioorg Med Chem Lett. 2014 Feb 1;24(3):963-8. doi: 10.1016/j.bmcl.2013.12.061. Epub 2013 Dec 21.

Abstract

As part of an effort to identify agonists of TRPV1, a peripheral sensory nerve ion channel, high throughput screening of the NIH Small Molecule Repository (SMR) collection identified MLS002174161, a pentacyclic benzodiazepine. A synthesis effort was initiated that ultimately afforded racemic seco analogs 12 of the SMR compound via a silver mediated intramolecular [3+2] cycloaddition of an azo-methine ylide generated from α-iminoamides 11. The cycloaddition set four contiguous stereocenters and, in some cases, also spontaneously afforded imides 13 from 12. The synthesis of compounds 12, the features that facilitated the conversion of 12-13, and their partial agonist activity against TRPV1 are discussed.

Keywords: Chronic pain; Intramolecular cycloaddition; Peripheral nerve ion channels; TRPV1 agonists.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, N.I.H., Intramural
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Amides / chemistry*
  • Azo Compounds / chemistry*
  • Benzodiazepinones / chemistry*
  • Capsaicin / chemistry
  • Cyclization
  • Cycloaddition Reaction
  • Heterocyclic Compounds, 4 or More Rings / chemistry*
  • Imines / chemistry*
  • Silver / chemistry*
  • TRPV Cation Channels / agonists*

Substances

  • Amides
  • Azo Compounds
  • Benzodiazepinones
  • Heterocyclic Compounds, 4 or More Rings
  • Imines
  • MLS002174161
  • TRPV Cation Channels
  • Silver
  • Capsaicin